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Register a new userValley and spin dynamics in monolayer MoS$_{2}$
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Valleytronics targets the exploitation of the additional degrees of freedom in materials where the energy of the carriers may assume several equal minimum values (valleys) at non-equivalent points of the reciprocal space. In single layers of transition metal dichalcogenides (TMDs) the lack of inversion symmetry, combined with a large spin-orbit interaction, leads to a conduction (valence) band with different spin-polarized minima (maxima) having equal energies. This offers the opportunity to manipulate information at the level of the charge (electrons or holes), spin (up or down) and crystal momentum (valley). Any implementation of these concepts, however, needs to consider the robustness of such degrees of freedom, which are deeply intertwined. Here we address the spin and valley relaxation dynamics of both electrons and holes with a combination of ultrafast optical spectroscopy techniques, and determine the individual characteristic relaxation times of charge, spin and valley in a MoS$_{2}$ monolayer. These results lay the foundations for understanding the mechanisms of spin and valley polarization loss in two-dimensional TMDs: spin/valley polarizations survive almost two-orders of magnitude longer for holes, where spin and valley dynamics are interlocked, than for electrons, where these degrees of freedom are decoupled. This may lead to novel approaches for the integration of materials with large spin-orbit in robust spintronic/valleytronic platforms.
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Valley pseudospin in two-dimensional (2D) transition-metal dichalcogenides (TMDs) allows optical control of spin-valley polarization and intervalley quantum coherence. Defect states in TMDs give rise to new exciton features and theoretically exhibit spin-valley polarization; however, experimental achievement of this phenomenon remains challenges. Here, we report unambiguous valley pseudospin of defect-bound localized excitons in CVD-grown monolayer MoS2; enhanced valley Zeeman splitting with an effective g-factor of -6.2 is observed. Our results reveal that all five d-orbitals and the increased effective electron mass contribute to the band shift of defect states, demonstrating a new physics of the magnetic responses of defect-bound localized excitons, strikingly different from that of A excitons. Our work paves the way for the manipulation of the spin-valley degrees of freedom through defects toward valleytronic devices.
Single layers of transition metal dichalcogenides (TMDs) are direct gap semiconductors with nondegenerate valley indices. An intriguing possibility for these materials is the use of their valley index as an alternate state variable. Several limitations to such a utility include strong, phonon-enabled intervalley scattering, as well as multiparticle interactions leading to multiple emission channels. We prepare single-layer WS$_{2}$ such that the photoluminescence is from either the neutral or charged exciton (trion). After excitation with circularly polarized light, the neutral exciton emission has zero polarization, however, the trion emission has a large polarization (28%) at room temperature. The trion emission also has a unique, non-monotonic temperature dependence that we show is a consequence of the multiparticle nature of the trion. This temperature dependence enables us to determine that coulomb assisted intervalley scattering, electron-hole radiative recombination, and a 3-particle Auger process are the dominant mechanisms at work in this system. Because this dependence involves trion systems, one can use gate voltages to modulate the polarization (or intensity) emitted from TMD structures.
We discuss here the effect of band nesting and topology on the spectrum of excitons in a single layer of MoS$_2$, a prototype transition metal dichalcogenide material. We solve for the single particle states using the ab initio based tight-binding model containing metal $d$ and sulfur $p$ orbitals. The metal orbitals contribution evolving from $K$ to $Gamma$ points results in conduction-valence band nesting and a set of second minima at $Q$ points in the conduction band. There are three $Q$ minima for each $K$ valley. We accurately solve the Bethe-Salpeter equation including both $K$ and $Q$ points and obtain ground and excited exciton states. We determine the effects of the electron-hole single particle energies including band nesting, direct and exchange screened Coulomb electron-hole interactions and resulting topological magnetic moments on the exciton spectrum. The ability to control different contributions combined with accurate calculations of the ground and excited exciton states allows for the determination of the importance of different contributions and a comparison with effective mass and $kcdot p$ massive Dirac fermion models.
WTe2 Weyl semimetal hosts the natural broken inversion symmetry and strong spin orbit coupling, making it promising for exotic spin/valley dynamics within a picosecond timescale. Here, we unveil an anisotropic ultrafast spin/valley dynamics in centimeter-scale, single-crystalline Td-WTe2 films using a femtosecond pump-probe technique at room temperature. We observe a transient (~0.8 ps) intra-valley transition and a subsequent polarization duration (~5 ps) during the whole spin/valley relaxation process. Furthermore, the relaxation exhibits the remarkable anisotropy of approximately six-fold and two-fold symmetries due to the intrinsic anisotropy along the crystalline orientation and the extrinsic matrix element effect, respectively. Our results offer a prospect for the ultrafast manipulation of spin/valleytronics in topological quantum materials for dissipationless high-speed spin/valleytronic devices.
Modern electronic devices heavily rely on the accurate control of charge and spin of electrons. The emergence of controllable valley degree of freedom brings new possibilities and presents a promising prospect towards valleytronics. Recently, valley excitation selected by chiral optical pumping has been observed in monolayer MoS2. In this work, we report polarized photoluminescence (PL) measurements for monolayer MoSe2, another member of the family of transition-metal-dichalcogenides (MX2), and observe drastic difference from the outcomes of MoS2. In particular, we identify a valley polarization (VP) up to 70% for B exciton, while that for A exciton is less than 3%. Besides, we also find a small but finite negative VP for A- trion. These results reveal several new intra- and inter-valley scattering processes which significantly affect valley polarization, hence provide new insights into exciton physics in monolayer MX2 and possible valleytronic applications.
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